Pub Date : 2025-12-17DOI: 10.1016/j.joule.2025.102169
Xiaohei Wu , Xinrong Yang , Bowen Chang , Rui Sun , Jie Min
Organic photovoltaics (OPVs) have witnessed significant advancements in device efficiency and operational stability, with single-junction cells exceeding 20% efficiency and over 10,000 h of lifetime. These improvements have been primarily driven by the rapid development of novel non-fullerene acceptors (NFAs) and their corresponding donor materials. Although relevant active layer materials are highly efficient and stable, their development largely relied on empirical trial-and-error approaches and the obsessive pursuit of performance metrics, with a limited understanding of the intricate structure-property relationships governing device performance, the suitable donor/acceptor (D/A) combinations, and component modulation. To bridge the gap between performance improvement and device practicality, this review examines and describes several important conceptual aspects of the emerging non-fullerene OPV systems that have provided fundamental insights into material design and D/A compatibility and further outlines the key challenges involved in NFA development and some perspectives along with useful material design guidelines. Looking forward, we will discuss some research directions in terms of NFA materials for further improving device collaboration performance.
{"title":"Material insights and challenges for organic photovoltaics based on non-fullerene acceptors","authors":"Xiaohei Wu , Xinrong Yang , Bowen Chang , Rui Sun , Jie Min","doi":"10.1016/j.joule.2025.102169","DOIUrl":"10.1016/j.joule.2025.102169","url":null,"abstract":"<div><div>Organic photovoltaics (OPVs) have witnessed significant advancements in device efficiency and operational stability, with single-junction cells exceeding 20% efficiency and over 10,000 h of lifetime. These improvements have been primarily driven by the rapid development of novel non-fullerene acceptors (NFAs) and their corresponding donor materials. Although relevant active layer materials are highly efficient and stable, their development largely relied on empirical trial-and-error approaches and the obsessive pursuit of performance metrics, with a limited understanding of the intricate structure-property relationships governing device performance, the suitable donor/acceptor (D/A) combinations, and component modulation. To bridge the gap between performance improvement and device practicality, this review examines and describes several important conceptual aspects of the emerging non-fullerene OPV systems that have provided fundamental insights into material design and D/A compatibility and further outlines the key challenges involved in NFA development and some perspectives along with useful material design guidelines. Looking forward, we will discuss some research directions in terms of NFA materials for further improving device collaboration performance.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 12","pages":"Article 102169"},"PeriodicalIF":35.4,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145306322","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-17DOI: 10.1016/j.joule.2025.102209
Ilhem Nadia Rabehi , Silvia Mariotti , Kenjiro Fukuda , Shin Young Lee , Dou Zhao , Penghui Ji , Shuai Yuan , Jiahao Zhang , Chenfeng Ding , Kirill Mitrofanov , Dominik Madea , Ryota Kabe , Tomoyuki Yokota , Luis K. Ono , Takao Someya , Yabing Qi
Perovskite materials are highly promising for ultra-flexible solar cells (u-FPSCs) due to their intrinsic mechanical flexibility and lightweight nature. Devices fabricated on substrates thinner than 10 μm are particularly attractive for emerging applications in wearable electronics and medical applications. Although their power conversion efficiency (PCE) approaches that of rigid glass-based devices, long-term stability remains a critical challenge. In this study, we show that the combination of nickel oxide and [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz) self-assembled monolayer as hole transport materials employed on indium tin oxide-coated transparent polyimide leads to a significant improvement of the device stability. This strategy enabled devices with PCEs of 20.3% and a stable power output for 1,200 h under inert conditions. Furthermore, the integration of a 15-nm Al₂O₃ humidity barrier preserved 90% of the PCE after 130 h in air, without compromising specific power (27.2 W g−1), establishing record ambient stability for u-FPSCs.
钙钛矿材料由于其固有的机械灵活性和轻质性，在超柔性太阳能电池（u-FPSCs）中具有很高的应用前景。在厚度小于10 μm的基板上制造的器件对于可穿戴电子产品和医疗应用中的新兴应用尤其具有吸引力。虽然它们的功率转换效率（PCE）接近刚性玻璃基器件，但长期稳定性仍然是一个关键挑战。在本研究中，我们证明了将氧化镍和[2-（9h -咔唑-9-基）乙基]膦酸（2PACz）自组装单层作为空穴传输材料应用于氧化铟锡涂层的透明聚酰亚胺上，可以显著提高器件的稳定性。该策略使器件的pce为20.3%，在惰性条件下稳定输出功率为1200小时。此外，集成的15纳米Al₂O₃湿度屏障在空气中放置130小时后保留了90%的PCE，而不影响比功率（27.2 W g−1），为u-FPSCs建立了创纪录的环境稳定性。
{"title":"Dual hole transport layer for ultra-flexible perovskite solar cells with unprecedented stability","authors":"Ilhem Nadia Rabehi , Silvia Mariotti , Kenjiro Fukuda , Shin Young Lee , Dou Zhao , Penghui Ji , Shuai Yuan , Jiahao Zhang , Chenfeng Ding , Kirill Mitrofanov , Dominik Madea , Ryota Kabe , Tomoyuki Yokota , Luis K. Ono , Takao Someya , Yabing Qi","doi":"10.1016/j.joule.2025.102209","DOIUrl":"10.1016/j.joule.2025.102209","url":null,"abstract":"<div><div>Perovskite materials are highly promising for ultra-flexible solar cells (u-FPSCs) due to their intrinsic mechanical flexibility and lightweight nature. Devices fabricated on substrates thinner than 10 μm are particularly attractive for emerging applications in wearable electronics and medical applications. Although their power conversion efficiency (PCE) approaches that of rigid glass-based devices, long-term stability remains a critical challenge. In this study, we show that the combination of nickel oxide and [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz) self-assembled monolayer as hole transport materials employed on indium tin oxide-coated transparent polyimide leads to a significant improvement of the device stability. This strategy enabled devices with PCEs of 20.3% and a stable power output for 1,200 h under inert conditions. Furthermore, the integration of a 15-nm Al₂O₃ humidity barrier preserved 90% of the PCE after 130 h in air, without compromising specific power (27.2 W g<sup>−1</sup>), establishing record ambient stability for u-FPSCs.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 12","pages":"Article 102209"},"PeriodicalIF":35.4,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145509898","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-17DOI: 10.1016/j.joule.2025.102216
Yongki Kim , Chanyong Lee , Gumin Kang , Youngbin Yoon , Jeonghyeon Ahn , Yong Ju Yun , Taemin Kim , Hae Jung Son , Beom Soo Joo , Yoonmook Kang , Hyungduk Ko , Myunghun Shin , Yongseok Jun
Urbanization and the climate crisis have driven the need for sustainable energy solutions, emphasizing the importance of building-integrated photovoltaic systems and transparent photovoltaic (TPV) modules. However, conventional TPVs face limitations in efficiency, scalability, and color rendering. This study introduces a hybrid solar window combining bifacial silicon solar cells with an optimized distributed Bragg reflector structure to address these challenges. The solar window selectively captures near-infrared light for power generation while transmitting visible light, achieving high transparency (average visible transmittance [AVT]: 75.6%) and superior color rendering (color rendering index [CRI]: 93.8). The experimental results demonstrate a power conversion efficiency of 8.29% and a light-utilization efficiency of 6.27%, exceeding the theoretical limits of non-selective TPVs. Furthermore, the solar window operates effectively under both sunlight and indoor lighting, showcasing its versatility. Its scalable, cost-effective design is compatible with existing building materials and represents a significant advancement toward sustainable urban infrastructure by merging energy generation with architectural functionality.
{"title":"Scalable hybrid solar window with high transparency, high efficiency, and superior color rendering","authors":"Yongki Kim , Chanyong Lee , Gumin Kang , Youngbin Yoon , Jeonghyeon Ahn , Yong Ju Yun , Taemin Kim , Hae Jung Son , Beom Soo Joo , Yoonmook Kang , Hyungduk Ko , Myunghun Shin , Yongseok Jun","doi":"10.1016/j.joule.2025.102216","DOIUrl":"10.1016/j.joule.2025.102216","url":null,"abstract":"<div><div>Urbanization and the climate crisis have driven the need for sustainable energy solutions, emphasizing the importance of building-integrated photovoltaic systems and transparent photovoltaic (TPV) modules. However, conventional TPVs face limitations in efficiency, scalability, and color rendering. This study introduces a hybrid solar window combining bifacial silicon solar cells with an optimized distributed Bragg reflector structure to address these challenges. The solar window selectively captures near-infrared light for power generation while transmitting visible light, achieving high transparency (average visible transmittance [AVT]: 75.6%) and superior color rendering (color rendering index [CRI]: 93.8). The experimental results demonstrate a power conversion efficiency of 8.29% and a light-utilization efficiency of 6.27%, exceeding the theoretical limits of non-selective TPVs. Furthermore, the solar window operates effectively under both sunlight and indoor lighting, showcasing its versatility. Its scalable, cost-effective design is compatible with existing building materials and represents a significant advancement toward sustainable urban infrastructure by merging energy generation with architectural functionality.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 12","pages":"Article 102216"},"PeriodicalIF":35.4,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145560442","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-17DOI: 10.1016/j.joule.2025.102213
Jiheon Kim , Suhas Mahesh , Hyeon Seok Lee , Roham Dorakhan , Yang Bai , Muhammad Imran , Kangming Li , Yutong Liu , Dongha Kim , Sungjin Park , Ali Shayesteh Zeraati , Hyun Sik Moon , Xiaodong Li , Fatemeh Arabyarmohammadi , Jehad Abed , Brook Wander , Chengqian Wu , Shijie Liu , Yurou Celine Xiao , Rui Kai Miao , David Sinton
Automated high-throughput experimentation combined with artificial intelligence holds the potential to accelerate materials discovery; however, utilizing this approach in heterogeneous electrocatalytic materials has been challenging. Here, we pursue the discovery of multi-element CO2 electrocatalysts by employing a machine learning algorithm that integrates human domain knowledge to enable on-the-fly editing of feature contributions. By combining this approach with an accelerated experimental platform, we navigate a 15-element space for CO2-to-C3 hydrocarbon electrosynthesis and achieve a ∼165× acceleration compared with a conventional screening approach—of which ∼33× comes from the new experimentation platform and a further ∼5× from incorporating human domain knowledge. We identify Cu0.98In0.02 as an effective catalyst for propylene electrosynthesis, achieving a production rate of 42 mmol gcat−1 h−1 in a 25 cm2 electrolyzer. Data mining on the 300-composition dataset reveals two distinct C–C coupling pathways toward C3 hydrocarbons—∗CO dimerization and ∗CHx-mediated coupling—with composition-dependent factors governing each pathway.
{"title":"Accelerated discovery of CO2-to-C3-hydrocarbon electrocatalysts with human-in-the-loop","authors":"Jiheon Kim , Suhas Mahesh , Hyeon Seok Lee , Roham Dorakhan , Yang Bai , Muhammad Imran , Kangming Li , Yutong Liu , Dongha Kim , Sungjin Park , Ali Shayesteh Zeraati , Hyun Sik Moon , Xiaodong Li , Fatemeh Arabyarmohammadi , Jehad Abed , Brook Wander , Chengqian Wu , Shijie Liu , Yurou Celine Xiao , Rui Kai Miao , David Sinton","doi":"10.1016/j.joule.2025.102213","DOIUrl":"10.1016/j.joule.2025.102213","url":null,"abstract":"<div><div>Automated high-throughput experimentation combined with artificial intelligence holds the potential to accelerate materials discovery; however, utilizing this approach in heterogeneous electrocatalytic materials has been challenging. Here, we pursue the discovery of multi-element CO<sub>2</sub> electrocatalysts by employing a machine learning algorithm that integrates human domain knowledge to enable on-the-fly editing of feature contributions. By combining this approach with an accelerated experimental platform, we navigate a 15-element space for CO<sub>2</sub>-to-C<sub>3</sub> hydrocarbon electrosynthesis and achieve a ∼165× acceleration compared with a conventional screening approach—of which ∼33× comes from the new experimentation platform and a further ∼5× from incorporating human domain knowledge. We identify Cu<sub>0.98</sub>In<sub>0.02</sub> as an effective catalyst for propylene electrosynthesis, achieving a production rate of 42 mmol g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup> in a 25 cm<sup>2</sup> electrolyzer. Data mining on the 300-composition dataset reveals two distinct C–C coupling pathways toward C<sub>3</sub> hydrocarbons—∗CO dimerization and ∗CH<sub><em>x</em></sub>-mediated coupling—with composition-dependent factors governing each pathway.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 12","pages":"Article 102213"},"PeriodicalIF":35.4,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145560441","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-17DOI: 10.1016/j.joule.2025.102212
Jin Wen , Yuxuan Liu , Yinke Wang , Guihao Wang , Ningchong Zheng , Wennan Ou , Jinyan Guo , Jiajia Hong , Yijia Guo , Wenchi Kong , Anh Dinh Bui , Haowen Luo , Hieu Nguyen , Yuefeng Nie , Ke Xiao , Ludong Li , Hairen Tan
The buried heterointerface between hole transport layers (HTLs) and perovskite films critically determines the efficiency and stability of scalable perovskite solar modules. While self-assembled monolayer (SAM)-based HTLs enable record efficiencies in spin-coated devices, scalable blade coating often induces micron-scale nanogaps at the SAM/perovskite interface, causing non-radiative recombination and mechanical degradation. Here, we introduce a buried integrating-passivation nanostructure (BIPN) atop SAM, where inorganic oxide nanoparticles are utilized as mechanical reinforcements and passivating molecules function as chemical stabilizers, anchoring onto spherical surfaces via hydrogen bonding. This design effectively alleviates interfacial stress and minimizes nanoscale gaps, simultaneously decreasing defects and strengthening the buried interface. As a result, blade-coated perovskite solar cells achieve a power conversion efficiency of 26.0% (certified at 25.7%), while minimodules (20.25 cm2 aperture) deliver 22.5% efficiency and show no degradation after 2,100 h under the International Summit on Organic Photovoltaic Stability (ISOS)-L-1 condition.
{"title":"Buried heterointerface reinforcement with passivation-integrated nanostructures for efficient and stable perovskite solar modules","authors":"Jin Wen , Yuxuan Liu , Yinke Wang , Guihao Wang , Ningchong Zheng , Wennan Ou , Jinyan Guo , Jiajia Hong , Yijia Guo , Wenchi Kong , Anh Dinh Bui , Haowen Luo , Hieu Nguyen , Yuefeng Nie , Ke Xiao , Ludong Li , Hairen Tan","doi":"10.1016/j.joule.2025.102212","DOIUrl":"10.1016/j.joule.2025.102212","url":null,"abstract":"<div><div>The buried heterointerface between hole transport layers (HTLs) and perovskite films critically determines the efficiency and stability of scalable perovskite solar modules. While self-assembled monolayer (SAM)-based HTLs enable record efficiencies in spin-coated devices, scalable blade coating often induces micron-scale nanogaps at the SAM/perovskite interface, causing non-radiative recombination and mechanical degradation. Here, we introduce a buried integrating-passivation nanostructure (BIPN) atop SAM, where inorganic oxide nanoparticles are utilized as mechanical reinforcements and passivating molecules function as chemical stabilizers, anchoring onto spherical surfaces via hydrogen bonding. This design effectively alleviates interfacial stress and minimizes nanoscale gaps, simultaneously decreasing defects and strengthening the buried interface. As a result, blade-coated perovskite solar cells achieve a power conversion efficiency of 26.0% (certified at 25.7%), while minimodules (20.25 cm<sup>2</sup> aperture) deliver 22.5% efficiency and show no degradation after 2,100 h under the International Summit on Organic Photovoltaic Stability (ISOS)-L-1 condition.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 12","pages":"Article 102212"},"PeriodicalIF":35.4,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145531813","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-17DOI: 10.1016/j.joule.2025.102201
Huaian Zhao , Lizhi Xiang , Binghan Cui , Qingjie Zhou , Jiannan Du , Sai Li , Zheng Liu , Geping Yin , Guokang Han , Chunyu Du
Understanding how inhomogeneous reactions evolve across the battery electrode is essential for deciphering degradation mechanisms and improving the performance of commercial batteries. However, operando tracking of such dynamic processes remains challenging due to the lack of non-destructive techniques with spatiotemporal resolution. Here, we develop a magnetic field mapping technique that enables operando monitoring of reaction inhomogeneities across spatial and temporal dimensions. This approach reveals a self-regulating dynamic feedback mechanism, which provides a theoretical framework for interpreting the spatiotemporal evolution of inhomogeneous reactions under different C-rates, battery designs, and environmental conditions. This method identifies otherwise inaccessible design defects by directly resolving their spatially localized influence on reaction dynamics. It also directly visualizes mechanically induced reaction bottlenecks and the redirection of reaction pathways, offering new operando insights into mechano-electrochemical coupling in batteries. These findings provide a new approach for understanding inhomogeneous degradation, guiding electrode design, and advancing multi-dimensional diagnostic strategies for commercial batteries.
{"title":"Operando mapping of the dynamic evolution of spatially inhomogeneous reactions in commercial batteries","authors":"Huaian Zhao , Lizhi Xiang , Binghan Cui , Qingjie Zhou , Jiannan Du , Sai Li , Zheng Liu , Geping Yin , Guokang Han , Chunyu Du","doi":"10.1016/j.joule.2025.102201","DOIUrl":"10.1016/j.joule.2025.102201","url":null,"abstract":"<div><div>Understanding how inhomogeneous reactions evolve across the battery electrode is essential for deciphering degradation mechanisms and improving the performance of commercial batteries. However, operando tracking of such dynamic processes remains challenging due to the lack of non-destructive techniques with spatiotemporal resolution. Here, we develop a magnetic field mapping technique that enables operando monitoring of reaction inhomogeneities across spatial and temporal dimensions. This approach reveals a self-regulating dynamic feedback mechanism, which provides a theoretical framework for interpreting the spatiotemporal evolution of inhomogeneous reactions under different C-rates, battery designs, and environmental conditions. This method identifies otherwise inaccessible design defects by directly resolving their spatially localized influence on reaction dynamics. It also directly visualizes mechanically induced reaction bottlenecks and the redirection of reaction pathways, offering new operando insights into mechano-electrochemical coupling in batteries. These findings provide a new approach for understanding inhomogeneous degradation, guiding electrode design, and advancing multi-dimensional diagnostic strategies for commercial batteries.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 12","pages":"Article 102201"},"PeriodicalIF":35.4,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145428016","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-17DOI: 10.1016/j.joule.2025.102197
Yuge Feng , Yoon Park , Shaoyun Hao , Chang Qiu , Shoukun Zhang , Zhou Yu , Zhiwei Fang , Tanguy Terlier , Chase Sellers , Khalid Mateen , Frank Despinois , Moussa Kane , Sibani Lisa Biswal , Haotian Wang
Conventional lithium-ion (Li-ion) battery recycling technologies, including pyrometallurgy and hydrometallurgy, require elevated temperatures or substantial chemical input to smelt or leach solid battery materials for Li separation. In this work, we leveraged the intrinsic delithiation chemistry of battery cathode materials as a separation mechanism and devised the zero-gap membrane electrode assembly (MEA) reactor for sustainable, scalable, and cost-effective Li recovery from waste LiFePO4 (LFP) battery black mass (BM). Our strategy achieved an impressive Li extraction Faradaic efficiency of 96.4%, yielding high-purity lithium hydroxide (LiOH) (∼99.0 wt %), and reduced energy consumption to as low as 103 kJ/kgBM. A 20 cm2 MEA reactor demonstrated stable operation for 1,000 h, processing ∼57 g of LFP BM and maintaining an average Li recovery rate of 89.8%. Additionally, the MEA reactor can be adapted to a roll-to-roll fashion to produce 0.98 M LiOH and can be extended to other cathode materials such as LiMn2O4, LiNi0.5Mn0.3Co0.2O2, and hybrid cathode materials.
{"title":"A direct electrochemical Li recovery from spent Li-ion battery cathode for high-purity lithium hydroxide feedstock","authors":"Yuge Feng , Yoon Park , Shaoyun Hao , Chang Qiu , Shoukun Zhang , Zhou Yu , Zhiwei Fang , Tanguy Terlier , Chase Sellers , Khalid Mateen , Frank Despinois , Moussa Kane , Sibani Lisa Biswal , Haotian Wang","doi":"10.1016/j.joule.2025.102197","DOIUrl":"10.1016/j.joule.2025.102197","url":null,"abstract":"<div><div>Conventional lithium-ion (Li-ion) battery recycling technologies, including pyrometallurgy and hydrometallurgy, require elevated temperatures or substantial chemical input to smelt or leach solid battery materials for Li separation. In this work, we leveraged the intrinsic delithiation chemistry of battery cathode materials as a separation mechanism and devised the zero-gap membrane electrode assembly (MEA) reactor for sustainable, scalable, and cost-effective Li recovery from waste LiFePO<sub>4</sub> (LFP) battery black mass (BM). Our strategy achieved an impressive Li extraction Faradaic efficiency of 96.4%, yielding high-purity lithium hydroxide (LiOH) (∼99.0 wt %), and reduced energy consumption to as low as 103 kJ/kg<sub>BM</sub>. A 20 cm<sup>2</sup> MEA reactor demonstrated stable operation for 1,000 h, processing ∼57 g of LFP BM and maintaining an average Li recovery rate of 89.8%. Additionally, the MEA reactor can be adapted to a roll-to-roll fashion to produce 0.98 M LiOH and can be extended to other cathode materials such as LiMn<sub>2</sub>O<sub>4</sub>, LiNi<sub>0.5</sub>Mn<sub>0.3</sub>Co<sub>0.2</sub>O<sub>2</sub>, and hybrid cathode materials.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 12","pages":"Article 102197"},"PeriodicalIF":35.4,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145455379","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-17DOI: 10.1016/j.joule.2025.102178
Chao-Yang Wang , Kaiqiang Qin , Nitesh Gupta
We examine the latest developments in all-climate batteries (ACBs) that enable efficient and resilient energy storage across extreme temperature ranges, e.g., from −50oC to +60oC. A figure of merit is presented to quantify where the current state of art, the latest advances and the future targets stand in this rapidly evolving field. We review two distinctive approaches driving power and stability improvements in both low- and high-temperature environments: materials innovation (particularly electrolyte formulations) and thermal actuation. It is found that there are still two-orders-of-magnitude gaps from the ACB target of high-temperature stability by materials innovation alone and that the material-thermal synergetic approach promises to attain the dual goals of ACBs for uncompromised power and stability at both low and high temperatures. Future research should be focused on developing heat-tolerant electrolytes and electrodes that can survive in 70oC–85oC environments.
{"title":"All-climate battery energy storage","authors":"Chao-Yang Wang , Kaiqiang Qin , Nitesh Gupta","doi":"10.1016/j.joule.2025.102178","DOIUrl":"10.1016/j.joule.2025.102178","url":null,"abstract":"<div><div>We examine the latest developments in all-climate batteries (ACBs) that enable efficient and resilient energy storage across extreme temperature ranges, e.g., from −50<sup>o</sup>C to +60<sup>o</sup>C. A figure of merit is presented to quantify where the current state of art, the latest advances and the future targets stand in this rapidly evolving field. We review two distinctive approaches driving power and stability improvements in both low- and high-temperature environments: materials innovation (particularly electrolyte formulations) and thermal actuation. It is found that there are still two-orders-of-magnitude gaps from the ACB target of high-temperature stability by materials innovation alone and that the material-thermal synergetic approach promises to attain the dual goals of ACBs for uncompromised power and stability at both low and high temperatures. Future research should be focused on developing heat-tolerant electrolytes and electrodes that can survive in 70<sup>o</sup>C–85<sup>o</sup>C environments.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 12","pages":"Article 102178"},"PeriodicalIF":35.4,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145442074","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-17DOI: 10.1016/j.joule.2025.102195
Do-Hyeon Kim , Young-Han Lee , Jeong-Myeong Yoon , Pugalenthiyar Thondaiman , Byung Chul Kim , In-Chul Choi , Jeong-Hee Choi , Ki-Joon Jeon , Cheol-Min Park
Silicon (Si) is an attractive high-capacity anode material for all-solid-state Li-ion batteries (ASSLIBs). However, significant volume change, low ionic/electronic conductivity, poor solid-electrolyte compatibility, and high stack pressure requirements limit its practical applications. To address these issues, we propose Li–Si compound anodes for ASSLIBs, selected based on formation energies predicted by density functional theory. Among the Li–Si compounds, Li7Si3 (Li2.33Si) exhibits the highest ionic conductivity along with high electronic conductivity, making it an ideal anode material. Moreover, its Li-storage mechanism (Li2.33 + αSi, 0 < α < 0.92) enables ultra-stable cycling with negligible volume change. A Li2.33Si|LiNi0.6Co0.2Mn0.2O2 full cell achieved high areal capacity, long cycle life, fast rate capability, wide operating temperature range, and low stack pressure, demonstrating that the Li2.33Si anode meets all the key requirements for high-performance anodes. Consequently, Li–Si compound anodes will serve as a key enabler for advancing ASSLIB technology, with the concept broadly extendable to other Li-based compounds.
{"title":"Li–Si compound anodes enabling high-performance all-solid-state Li-ion batteries","authors":"Do-Hyeon Kim , Young-Han Lee , Jeong-Myeong Yoon , Pugalenthiyar Thondaiman , Byung Chul Kim , In-Chul Choi , Jeong-Hee Choi , Ki-Joon Jeon , Cheol-Min Park","doi":"10.1016/j.joule.2025.102195","DOIUrl":"10.1016/j.joule.2025.102195","url":null,"abstract":"<div><div>Silicon (Si) is an attractive high-capacity anode material for all-solid-state Li-ion batteries (ASSLIBs). However, significant volume change, low ionic/electronic conductivity, poor solid-electrolyte compatibility, and high stack pressure requirements limit its practical applications. To address these issues, we propose Li–Si compound anodes for ASSLIBs, selected based on formation energies predicted by density functional theory. Among the Li–Si compounds, Li<sub>7</sub>Si<sub>3</sub> (Li<sub>2.33</sub>Si) exhibits the highest ionic conductivity along with high electronic conductivity, making it an ideal anode material. Moreover, its Li-storage mechanism (Li<sub>2.33 + α</sub>Si, 0 < α < 0.92) enables ultra-stable cycling with negligible volume change. A Li<sub>2.33</sub>Si|LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> full cell achieved high areal capacity, long cycle life, fast rate capability, wide operating temperature range, and low stack pressure, demonstrating that the Li<sub>2.33</sub>Si anode meets all the key requirements for high-performance anodes. Consequently, Li–Si compound anodes will serve as a key enabler for advancing ASSLIB technology, with the concept broadly extendable to other Li-based compounds.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 12","pages":"Article 102195"},"PeriodicalIF":35.4,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145455378","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-17DOI: 10.1016/j.joule.2025.102199
Qin Peng , Haokai Xu , Yuan He , Yutong Jiang , Zhenglong Wu , Yudong Zhang , Xun Zhu , Jun Li , Wei Yang , Qiang Liao
The performance of gas diffusion electrodes (GDEs) with high catalyst loadings for multiphase electrochemical conversion is often compromised by sluggish mass transport arising from competing gas-liquid transport through the tortuous pore structure. Inspired by ridge-furrow irrigation in agriculture, we propose an aligned-pore engineering strategy to decouple the competing transport processes by leveraging pore-size-dependent capillary forces and enrich abundant three-phase interfaces (TPIs) in GDEs. Compared with a conventional electrode, the engineered electrode has a 46% lower mass transport impedance and 1.96-fold more TPIs. The optimized electrode delivers a maximum power (current) density of 85.5 mW cm−2 (634.4 mA cm−2), which is 82% (83%) higher than that of the conventional electrode, standing out as the highest reported for air-breathing membraneless direct formate fuel cells (DFFCs). The universality of this strategy is validated for direct methanol fuel cells, zinc-air batteries, and CO2 electrolysis cells, demonstrating broad applicability for high-performance GDEs.
高催化剂负载的气体扩散电极（GDEs）的多相电化学转化性能经常受到通过弯曲孔隙结构的气液相互竞争所引起的缓慢的质量传递的影响。受农业垄沟灌溉的启发，我们提出了一种对齐孔工程策略，通过利用孔径依赖的毛细力和丰富的GDEs三相界面（tpi）来解耦竞争的运输过程。与传统电极相比，工程电极的质量传输阻抗降低了46%，tpi增加了1.96倍。优化后的电极提供的最大功率（电流）密度为85.5 mW cm - 2 (634.4 mA cm - 2)，比传统电极高82%(83%)，是目前报道的呼吸式无膜直接甲酸盐燃料电池（DFFCs）中最高的。该策略的通用性在直接甲醇燃料电池、锌空气电池和二氧化碳电解电池中得到了验证，证明了高性能gde的广泛适用性。
{"title":"Aligned-pore engineering: Decoupling gas-liquid transport in gas diffusion electrodes","authors":"Qin Peng , Haokai Xu , Yuan He , Yutong Jiang , Zhenglong Wu , Yudong Zhang , Xun Zhu , Jun Li , Wei Yang , Qiang Liao","doi":"10.1016/j.joule.2025.102199","DOIUrl":"10.1016/j.joule.2025.102199","url":null,"abstract":"<div><div>The performance of gas diffusion electrodes (GDEs) with high catalyst loadings for multiphase electrochemical conversion is often compromised by sluggish mass transport arising from competing gas-liquid transport through the tortuous pore structure. Inspired by ridge-furrow irrigation in agriculture, we propose an aligned-pore engineering strategy to decouple the competing transport processes by leveraging pore-size-dependent capillary forces and enrich abundant three-phase interfaces (TPIs) in GDEs. Compared with a conventional electrode, the engineered electrode has a 46% lower mass transport impedance and 1.96-fold more TPIs. The optimized electrode delivers a maximum power (current) density of 85.5 mW cm<sup>−2</sup> (634.4 mA cm<sup>−2</sup>), which is 82% (83%) higher than that of the conventional electrode, standing out as the highest reported for air-breathing membraneless direct formate fuel cells (DFFCs). The universality of this strategy is validated for direct methanol fuel cells, zinc-air batteries, and CO<sub>2</sub> electrolysis cells, demonstrating broad applicability for high-performance GDEs.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 12","pages":"Article 102199"},"PeriodicalIF":35.4,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145478254","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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